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The impact of oxygen-clustering on the transformation of electrochemically-derived graphite oxide framework

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dc.abstract.enOxygen-clustering in graphene oxide is the activated process of diffusion of oxygen functionalities: hydroxyls and epoxides, to form clusters and to trigger sp2 percolation, a key element for electrical conductivity. Impact of oxygen-clustering is thoroughly analyzed in electrochemically-derived graphite oxide (EGO), amine-functionalized frameworks (EGOF), and their pyrolyzed forms. Amine pillars within EGOF were suspected to amplify oxygen-clustering in EGOF as onset temperature of thermal decomposition was smaller in EGOF than in EGO. Thermochemical analysis proves that pillars within EGOF significantly augment oxygen-clustering aiding the reduction mechanism as inferred by the activation energy of thermal decomposition. Defective oxygen-clustering mechanism is evidenced using multiple techniques, including XRD, and is harnessed to enhance nitrogen doping. The pyrolytic morphological transformation from lamellae of EGOF into ravioli is revealed through SEM. A labyrinthic network of array prismatic dislocations provides stability to pyrolyzed EGOF ravioli whilst confining long chains of electron delocalization (localized π-orbitals), as unprecedently confirmed by HR-TEM/EELS and conductive AFM (C-AFM). Oxygen-clustering not only improves nitrogen doping in ravioli, but also improves density of array prismatic dislocations, which ultimately boosts Faradaic redox activity as observed in cyclic voltammetry (CV). Results show that Faradaic response originating from redox-active nitrogen groups predominantly relies on abundance of extended localized π-orbitals, which are geometrically and chemically confined within ravioli array prismatic dislocations. Our first-of-a-kind HR-TEM/EELS, C-AFM, and CV comparative and correlative analysis of pyrolyzed forms of EGO, EGOF, and their oxygen-clustered derivatives, confirms emergent role of confined electron delocalizations in amplifying Faradaic redox activity.
dc.affiliationWydział Nauk o Żywności i Żywieniu
dc.affiliation.instituteKatedra Fizyki i Biofizyki
dc.contributor.authorSubrati, Ahmed
dc.contributor.authorGurzęda, Bartosz
dc.contributor.authorJeżowski, Pawel
dc.contributor.authorKościński, Mikołaj
dc.contributor.authorNowaczyk, Grzegorz
dc.contributor.authorKempiński, Mateusz
dc.contributor.authorFlorczak, Patryk
dc.contributor.authorPeplińska, Barbara
dc.contributor.authorJarek, Marcin
dc.contributor.authorAl Wahedi, Yasser
dc.contributor.authorKempiński, Wojciech
dc.contributor.authorSmardz, Leslaw
dc.contributor.authorKrawczyk, Piotr
dc.date.accessioned2025-07-21T12:24:41Z
dc.date.available2025-07-21T12:24:41Z
dc.date.issued2024
dc.description.bibliographyil., bibliogr.
dc.description.financepublication_nocost
dc.description.financecost0.00
dc.description.if11,6
dc.description.number25 January 2024
dc.description.points140
dc.description.volume217
dc.identifier.doi10.1016/j.carbon.2023.118641
dc.identifier.eissn1873-3891
dc.identifier.issn0008-6223
dc.identifier.urihttps://sciencerep.up.poznan.pl/handle/item/3913
dc.languageen
dc.pbn.affiliationfood and nutrition technology
dc.relation.ispartofCarbon
dc.relation.pagesart. 118641
dc.rightsClosedAccess
dc.sciencecloudsend
dc.subject.engraphite oxide framework
dc.subject.enoxygen-clustering
dc.subject.enarray prismatic dislocation
dc.subject.ennitrogen doping
dc.subject.enconfined electron delocalization
dc.subject.enfast faradaic reaction
dc.titleThe impact of oxygen-clustering on the transformation of electrochemically-derived graphite oxide framework
dc.typeJournalArticle
dspace.entity.typePublication
oaire.citation.volume217